US3056646A - Method of effecting the catalytic contact of gases containing oxygen and methane - Google Patents
Method of effecting the catalytic contact of gases containing oxygen and methane Download PDFInfo
- Publication number
- US3056646A US3056646A US826934A US82693459A US3056646A US 3056646 A US3056646 A US 3056646A US 826934 A US826934 A US 826934A US 82693459 A US82693459 A US 82693459A US 3056646 A US3056646 A US 3056646A
- Authority
- US
- United States
- Prior art keywords
- methane
- oxygen
- catalyst
- admixture
- percent
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
Links
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B21/00—Nitrogen; Compounds thereof
- C01B21/04—Purification or separation of nitrogen
- C01B21/0405—Purification or separation processes
- C01B21/0411—Chemical processing only
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B23/00—Noble gases; Compounds thereof
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/50—Carbon dioxide
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
- C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/03—Precipitation; Co-precipitation
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
- C01B2210/0043—Impurity removed
- C01B2210/0045—Oxygen
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
- C01B2210/0043—Impurity removed
- C01B2210/0068—Organic compounds
- C01B2210/007—Hydrocarbons
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/20—Capture or disposal of greenhouse gases of methane
Definitions
- This invention relates to a process for effecting combustion reactions of oxygen-containing gases and, more particularly, relates to specific fuel-catalyst combinations which afford low ignition or kindling temperatures of methane in admixture with oxygen-containing gases.
- catalysts and process conditions are provided which achieve these desirable results in a practical, efficient and economical manner.
- the invention is, however, not limited to these specific objectives.
- a catalyst One of the most important functions of .a catalyst is that it promotes the desired reactions at temperatures appreciably lower than those at which the non-catalytic reactions occur at a practical rate. In the case of methane oxidation, this is an especially important consideration, since experience has shown that, of all hydrocarbons, it is the most difficult to ignite. On the other hand, methane is also often the cheapest fuel available to an industrial user, being the principal constituent of natural gas. These two facts thus make it economically important to find means for igniting or initiating the methane-oxygen reaction at the lowest possible temperature.
- supported platinum group metal catalysts as well as silver are especially eliective for promoting the oxygen methane reaction.
- the most effective metals are palladium, platinium, ruthenium, rhodium and iridium and mixtures thereof. From the standpoint of low ignition temperature, the most active of these metals is rhodium, although palladium is almost as active; under certain conditions, 0.5 percent palladium metal supported on activated alumina pellets etiects methane oxidation at an initial gas temperature of 2812 C.
- the ignition temperature is, to some extent, a function of gas composition and other operating variables, as will be noted from the examples below.
- a further important characteristic of catalysts is the completeness with which they eifect the desired reaction. Using completeness as the criterion, the platinum group metals and silver are again the most efifective.
- the catalytic process of the invention is used to remove oxygen from gas streams by the oxidation of methane, purified streams result which contain only a few parts per million of oxygen, and methane concentration can be reduced to the part-per-million level in gas streams 3,050,546 Patented Get. 2, i062 ice using a very slight excess of oxygen. Both types of catalytic process are illustrated in the examples below.
- the catalysts which may be used in the process of the invention are palladium, platinum, ruthenium, rhodium, iridium or osmium, per se, or in admixture with each other, and/or supported on suitable carriers.
- the supported catalysts may contain from about 0.05 to 5 percent, by weight,-of the catalytic metal, although 0.5 percent is a metal content which produces excellent results from the standpoint of both economy and activity.
- the catalyst may be supported on suitable supports such as activated alumina, silica, silica gel, diatomaceous earth and other similar catalyst supports, and the supported.
- catalyst may be prepared in any suitable manner, e.g. by treating the carrier or support with a solution of a suitable metal compound and then reducing the metal compound to metal.
- the catalyst support may be in the form of granules, pellets, or powder.
- the catalysts of the invention will ignite methaneoxygen mixtures at temperatures as low as 271 C., and are operable at temperatures in the range up to 900 C. and higher. In general, the higher the operating temperature, the shorter will be the catalyst life and the more difficult will be subsequent ignition after catalyst cooling.
- the space velocity may be in the range of about to 200,000 standard volumes of gas per volume of catalyst per hour, and a space velocity in the range of about 2,000 to 100,000 standard volumes per volume per hour is preferred.
- the reaction pressure may be in the range of atmospheric to about 500 p.s.i.g. or higher. Pressure limitations are imposed by the strength limits of catalyst vessels rather than by any fundamental properties of the catalysts themselves.
- the deficient compound is removed with a slight excess of the other.
- the methane and oxygen may be in admixture with any of a large number of inert gases, such as nitrogen, argon, helium, neon, carbon dioxide and the like; the streams may be initially dry or saturated with water vapor.
- An upper limit on the oxygen or methane removable in a single pass over the catalyst arises from the minimum and maximum temperatures at which a given catalyst can operate. Generally, this consideration will limit the oxygen removable per pass to about 4 percent, or the methane to 2 percent, by volume, in nitrogen, or to somewhat dilierent values in diluent gases having specific heats different from that of nitrogen.
- engineering design can overcome this limitation by providing, for example, either for re-cycling of gas so as to maintain the inlet composition at the desired value, or by passing the full gas stream through two or more stages of catalyst, with intermediate cooling.
- the process of the invention can be utilized to treat gases having very high concentrations of methane and/ or oxygen.
- EXAMPLE I A gas mixture of 1.5 percent methane, 3 percent oxygen, and 95.5 percent nitrogen was passed, at the rate of 10 cubic feet per hour, through a bed containing 2.5 grams of catalyst pellets, at atmospheric pressure. The temperature was gradually raised until the catalyst temperature showed a sudden increase due to combustion, and the temperature at which the sudden. increase occurred was taken as the ignition point. In another series of experiments, conditions were the same, except that a gas containing 21 percent oxygen was employed. The results of the catalyst evaluations are as follows:
- Atmosphere Rh Pd Pd Rh Ir Ru Ru Ir Pt Pt Economic as Well as technical factors Will affect the choice of catalyst in individual cases and, thus, palladium may often be chosen to operate in a neutral or reducing atmosphere, where rhodium shows a slight technical superiority.
- EXAMPLE III A series of experiments was conducted to remove oxygen from a nitrogen stream by catalytic reaction of the oxygen with methane. A mixture containing 0.33 percent oxygen, by volume, in nitrogen, was mixed with methane and passed over ml. of 0.5 percent palladium supported on activated alumina at atmospheric pressure. Good oxygen removal was obtained at flow rates in the 4 range of 10,000 to 20,000 ml. of gas per hour per gram of catalyst, under laboratory conditions.
- EXAMPLE IV A series of experiments was conducted similar to the experiments of Example III above. However, the stream to be purified consisted of 0.30 percent oxygen, 11.4 percent carbon dioxide, 2.3-2.5 percent water vapor and the balance was nitrogen. Five grams of 0.5 percent palladium on activated alumina catalyst were used and the stream passed through the bed at flow rates of to 300 liters per hour. Good oxygen removal was found at space velocities as high as 60,000.
- the carbon monoxide concentration in the eflluent was between 100 and 200 parts per million in experiment 1, and about 200 parts per million in experiment 2.
- EXAMPLE V An experiment was conducted in order to remove methane from an inert gas stream by reaction with oxygen, the carbon dioxide and water formed being readily removable by conventional means.
- the catalyst was 0.5 percent palladium on activated alumina pellets, and the gas stream was argon to which carefully measured quantities of methane, carbon monoxide and oxygen had been added.
- the catalyst charge five grams, was placed in an 0.82" internal diameter stainless steel reactor, which was operated at a gas pressure of 35 p.s.i.g. The gas was passed through the catalyst bed, which was heated to the desired temperatures, and the catalyst efiluent was analyzed for total combustible carbon (the sum of carbon monoxide and methane) at various conditions. The results are tabulated below for an inlet gas containing 50 parts per million carbon monoxide, 50 parts per million of methane, and 1000 parts per million of oxygen.
- a process for effecting the ignition and combustion of a gaseous mixture consisting essentially of oxygen, methane and inert gases which comprises adding a fuel consisting essentially of methane to a gaseous mixture consisting essentially of oxygen and inert gases, and contacting the resulting gaseous admixture at a temperature above the ignition temperature of said admixture but not in excess of 400 C. with a catalyst selected from the group consisting of rhodium and rhodium in admixture with another platinum group metal, thereby igniting the gaseous admixture and eifecting the combustion thereof.
- a process for effecting the ignition and combustion of a gaseous mixture consisting essentially of oxygen, methane and inert gases which comprises adding a fuel consisting essentially of methane to a gaseous mixture consisting essentially of oxygen and inert gases, and contacting the resulting gaseous admixture with a catalyst selected from the group consisting of rhodium and rhodium in admixture with another platinum group metal, thereby igniting the gaseous admixture at a temperature in the range of from 271 C. to 400 C.
- space velocity is in the range of about to 200,000 s.c.f.h./c.f.
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Analytical Chemistry (AREA)
- Inorganic Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Combustion & Propulsion (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Environmental & Geological Engineering (AREA)
- Catalysts (AREA)
Priority Applications (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US826934A US3056646A (en) | 1959-07-14 | 1959-07-14 | Method of effecting the catalytic contact of gases containing oxygen and methane |
FR832063A FR1271090A (fr) | 1959-07-14 | 1960-07-05 | Procédé de combustion catalytique de gaz |
GB24448/60A GB935951A (en) | 1959-07-14 | 1960-07-13 | A process for removing methane or oxygen from a gas containing the same |
DEE19598A DE1151247B (de) | 1959-07-14 | 1960-07-13 | Verfahren zum Zuenden und Verbrennen von Gasgemischen, die Sauerstoff und Methan enthalten |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US826934A US3056646A (en) | 1959-07-14 | 1959-07-14 | Method of effecting the catalytic contact of gases containing oxygen and methane |
Publications (1)
Publication Number | Publication Date |
---|---|
US3056646A true US3056646A (en) | 1962-10-02 |
Family
ID=25247890
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US826934A Expired - Lifetime US3056646A (en) | 1959-07-14 | 1959-07-14 | Method of effecting the catalytic contact of gases containing oxygen and methane |
Country Status (4)
Country | Link |
---|---|
US (1) | US3056646A (de) |
DE (1) | DE1151247B (de) |
FR (1) | FR1271090A (de) |
GB (1) | GB935951A (de) |
Cited By (12)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3806582A (en) * | 1969-09-16 | 1974-04-23 | Johnson Matthey Co Ltd | Catalytic reactions |
WO1993018347A1 (en) * | 1992-03-13 | 1993-09-16 | Engelhard Corporation | Catalytic combustion process using supported palladium oxide catalysts |
US5384300A (en) * | 1993-04-28 | 1995-01-24 | Engelhard Corporation | Stabilized catalyst carrier and improved carrier configuration for catalytic combustion system |
US5474441A (en) * | 1989-08-22 | 1995-12-12 | Engelhard Corporation | Catalyst configuration for catalytic combustion systems |
US5551239A (en) * | 1993-03-01 | 1996-09-03 | Engelhard Corporation | Catalytic combustion system including a separator body |
US5552360A (en) * | 1993-03-04 | 1996-09-03 | Engelhard Corporation | Substrate configuration for catalytic combustion systems |
US5863851A (en) * | 1991-04-12 | 1999-01-26 | Engelhard Corporation | Combustion catalysts containing binary oxides and processes using the same |
US6015285A (en) * | 1998-01-30 | 2000-01-18 | Gas Research Institute | Catalytic combustion process |
US20060292051A1 (en) * | 2001-12-27 | 2006-12-28 | Nissan Motor Co., Ltd. | Exhaust gas purifying method for fuel cell vehicle and exhaust gas purifying system for fuel cell vehicle |
US20090178901A1 (en) * | 2006-06-01 | 2009-07-16 | As Techno-Track | Guidance unit for conveyor belt |
WO2017009243A1 (de) * | 2015-07-13 | 2017-01-19 | Wacker Chemie Ag | Verfahren zur entfernung von sauerstoff aus einem kohlenwasserstoff und sauerstoff enthaltenden gasgemisch |
US10159172B2 (en) | 2013-03-15 | 2018-12-25 | Textron Innovations Inc. | Tine holding apparatus and method for aerating soil |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR3096900B1 (fr) * | 2019-06-06 | 2021-10-01 | Air Liquide | Procédé et unité de purification d’hélium |
CN110721707B (zh) * | 2019-10-30 | 2022-07-12 | 大连凯特利催化工程技术有限公司 | 一种合成气低温脱氧催化剂及其制备和应用 |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US1934838A (en) * | 1930-04-14 | 1933-11-14 | Ig Farbenindustrie Ag | Production of hydrocyanic acid |
US1960212A (en) * | 1927-02-03 | 1934-05-22 | Empire Oil & Refining Company | Removal of oxygen from combustible gases |
US2776317A (en) * | 1952-03-25 | 1957-01-01 | Dresser Operations Inc | Partial oxidation of hydrocarbons in the presence of sulfur dioxide |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE716852C (de) * | 1937-01-09 | 1942-01-30 | Heraeus Gmbh W C | Katalysator zur flammenlosen Verbrennung |
-
1959
- 1959-07-14 US US826934A patent/US3056646A/en not_active Expired - Lifetime
-
1960
- 1960-07-05 FR FR832063A patent/FR1271090A/fr not_active Expired
- 1960-07-13 GB GB24448/60A patent/GB935951A/en not_active Expired
- 1960-07-13 DE DEE19598A patent/DE1151247B/de active Pending
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US1960212A (en) * | 1927-02-03 | 1934-05-22 | Empire Oil & Refining Company | Removal of oxygen from combustible gases |
US1934838A (en) * | 1930-04-14 | 1933-11-14 | Ig Farbenindustrie Ag | Production of hydrocyanic acid |
US2776317A (en) * | 1952-03-25 | 1957-01-01 | Dresser Operations Inc | Partial oxidation of hydrocarbons in the presence of sulfur dioxide |
Cited By (19)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3806582A (en) * | 1969-09-16 | 1974-04-23 | Johnson Matthey Co Ltd | Catalytic reactions |
US5474441A (en) * | 1989-08-22 | 1995-12-12 | Engelhard Corporation | Catalyst configuration for catalytic combustion systems |
US5863851A (en) * | 1991-04-12 | 1999-01-26 | Engelhard Corporation | Combustion catalysts containing binary oxides and processes using the same |
EP0886107A2 (de) | 1992-03-13 | 1998-12-23 | Engelhard Corporation | Katalytisches verbrennungsverfahren mit palladiumoxyd-trägerkatalysatoren |
WO1993018347A1 (en) * | 1992-03-13 | 1993-09-16 | Engelhard Corporation | Catalytic combustion process using supported palladium oxide catalysts |
US5551239A (en) * | 1993-03-01 | 1996-09-03 | Engelhard Corporation | Catalytic combustion system including a separator body |
US5622041A (en) * | 1993-03-01 | 1997-04-22 | Engelhard Corporation | Catalytic combustion system including a separator body |
US5552360A (en) * | 1993-03-04 | 1996-09-03 | Engelhard Corporation | Substrate configuration for catalytic combustion systems |
US5509798A (en) * | 1993-04-28 | 1996-04-23 | Engelhard Corporation | Stabilized catalyst carrier and improved carrier configuration for catalytic combustion system |
US5384300A (en) * | 1993-04-28 | 1995-01-24 | Engelhard Corporation | Stabilized catalyst carrier and improved carrier configuration for catalytic combustion system |
US6015285A (en) * | 1998-01-30 | 2000-01-18 | Gas Research Institute | Catalytic combustion process |
US20060292051A1 (en) * | 2001-12-27 | 2006-12-28 | Nissan Motor Co., Ltd. | Exhaust gas purifying method for fuel cell vehicle and exhaust gas purifying system for fuel cell vehicle |
US20080219907A1 (en) * | 2001-12-27 | 2008-09-11 | Nissan Motor Co., Ltd | Exhaust gas purifying method for fuel cell vehicle and exhaust gas purifying system for fuel cell vehicle |
US7572422B2 (en) | 2001-12-27 | 2009-08-11 | Nissan Motor Co., Ltd. | Exhaust gas purifying method for fuel cell vehicle and exhaust gas purifying system for fuel cell vehicle |
US20090178901A1 (en) * | 2006-06-01 | 2009-07-16 | As Techno-Track | Guidance unit for conveyor belt |
US7669709B2 (en) * | 2006-06-01 | 2010-03-02 | Hovstoe Kenneth | Guidance unit for conveyor belt |
US10159172B2 (en) | 2013-03-15 | 2018-12-25 | Textron Innovations Inc. | Tine holding apparatus and method for aerating soil |
WO2017009243A1 (de) * | 2015-07-13 | 2017-01-19 | Wacker Chemie Ag | Verfahren zur entfernung von sauerstoff aus einem kohlenwasserstoff und sauerstoff enthaltenden gasgemisch |
US10363524B2 (en) | 2015-07-13 | 2019-07-30 | Wacker Chemie Ag | Process for removing oxygen from a gas mixture comprising hydrocarbon and oxygen |
Also Published As
Publication number | Publication date |
---|---|
GB935951A (en) | 1963-09-04 |
DE1151247B (de) | 1963-07-11 |
FR1271090A (fr) | 1961-09-08 |
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